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Studies of photoinduced molecular dynamics using a fast imaging sensor

Author: Craig S Slater
Publisher: Cham : Springer, [2016] ©2016
Series: Springer theses.
Edition/Format:   eBook : Document : EnglishView all editions and formats
Database:WorldCat
Summary:
The work presented in this thesis involves a number of sophisticated experiments highlighting novel applications of the Pixel Imaging Mass Spectrometry (PImMS) camera in the field of photoinduced molecular dynamics. This approach represents the union of a new enabling technology (a multiple memory register, CMOS-based pixel detector) with several modern chemical physics approaches and represents a significant leap  Read more...
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Genre/Form: Electronic books
Additional Physical Format: (OCoLC)918590427
Material Type: Document, Internet resource
Document Type: Internet Resource, Computer File
All Authors / Contributors: Craig S Slater
ISBN: 9783319245171 3319245171
OCLC Number: 925478344
Description: 1 online resource.
Contents: Parts of this thesis have been published in the following journal articles:; Supervisor's Foreword; Acknowledgements; Contents; 1 Introduction and Motivation; 1.1 Motivation; 1.2 Photoinduced Molecular Dynamics; 1.2.1 Molecular Photodissociation; 1.2.2 Coulomb Explosion; 1.3 Femtochemistry; 1.3.1 Strong Field Control of Molecular Motion; 1.4 Position-Sensitive Coincidence Spectroscopy; 1.5 Ion Imaging; 1.5.1 Velocity-Mapping; 1.6 Fast Detectors in Ion Imaging; 1.6.1 Microchannel Plates; 1.6.2 Anode Readout Technologies; 1.6.3 Pixelated Silicon Detectors; 1.7 Outline of This Thesis; References 2 Experimental Techniques and Methods of Data Analysis2.1 Experimental Principles; 2.2 The Oxford VMI Spectrometer; 2.2.1 Overview; 2.2.2 Ion Optics; 2.2.3 Detector; 2.2.4 Optical Systems; 2.2.5 Reagent Sources; 2.3 The Aarhus VMI Spectrometer; 2.3.1 Overview; 2.3.2 Molecular Beam Source; 2.3.3 Electrostatic Deflector; 2.3.4 Optical Systems; 2.3.5 Nanosecond Laser System; 2.3.6 Femtosecond Laser System; 2.3.7 Reagent Source; 2.4 Velocity-Map Image Analysis; 2.5 The PImMS Camera; 2.5.1 CMOS Technology; 2.5.2 PImMS Pixel Architecture and Functionality; 2.5.3 Post-Processing 2.5.4 Characterisation and PerformanceReferences; 3 Three-Dimensional Velocity-Map Imaging; 3.1 Imaging the Newton-Sphere; 3.1.1 Ion Extraction Methods; 3.2 Simulations; 3.3 Experimental Results; 3.3.1 Experimental Conditions; 3.3.2 PImMS Data Processing; 3.3.3 PImMS Images; 3.4 Discussion; References; 4 Pulsed-Field Electron-Ion Imaging; 4.1 Introduction; 4.2 Simulations; 4.3 Experimental Images; 4.3.1 CCD Images; 4.3.2 PImMS Images; 4.4 Measurement of the Detection Efficiency; 4.5 Discussion; References; 5 Principles of Coulomb Explosion Imaging; 5.1 Background and Motivation 5.2 Coulomb Explosion Imaging5.2.1 Methods of Ionisation; 5.2.2 Ionisation by Intense Laser Fields; 5.3 Molecular Alignment; 5.3.1 Principles of Laser-Induced Alignment; 5.3.2 Non-adiabatic Alignment; 5.3.3 3D Alignment; 5.4 Summary; References; 6 Investigations of Coulomb Explosion Dynamics; 6.1 Introduction; 6.1.1 The Molecule; 6.1.2 Experimental Details; 6.2 Adiabatic Alignment; 6.3 Time-of-Flight Spectra; 6.3.1 General Details of the Spectra; 6.3.2 Ion Yields; 6.3.3 Time-of-Flight Covariance; 6.4 Recoil Frame Covariance Images; 6.4.1 Overview of Covariance Images 6.4.2 Detailed Analysis of Selected Covariance Images6.5 Classical Simulations of Coulomb Explosion; 6.5.1 Computational Details; 6.5.2 Details of the Ion Trajectories; 6.5.3 Comparison to Experimental Data; 6.6 Simulation of Experimental Data; 6.6.1 Details of the Simulations; 6.6.2 Simulation Results; 6.7 Summary; References; 7 Time-Resolved Studies of Induced Torsional Motion; 7.1 Introduction; 7.2 Experimental Details; 7.3 Single Kick Torsional Dynamics; 7.3.1 Theoretical Treatment; 7.3.2 Alignment Dynamics; 7.3.3 Time-Resolved Torsional Motion
Series Title: Springer theses.
Responsibility: Craig S. Slater.
More information:

Abstract:

The work presented in this thesis involves a number of sophisticated experiments highlighting novel applications of the Pixel Imaging Mass Spectrometry (PImMS) camera in the field of photoinduced molecular dynamics. This approach represents the union of a new enabling technology (a multiple memory register, CMOS-based pixel detector) with several modern chemical physics approaches and represents a significant leap forward in capabilities. Applications demonstrated include three-dimensional imaging of photofragment Newton spheres, simultaneous electron-ion detection using a single sensor, and ion-ion velocity correlation measurements that open the door to novel covariance imaging experiments. When combined with Coulomb explosion imaging, such an approach is demonstrated to allow the measurement of molecular structure and motion on a femtosecond timescale. This is illustrated through the controlled photoexcitation of torsional motion in biphenyl molecules and the subsequent real-time measurement of the torsional angle.

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